Engineering the Cu(0)-Co₂C Interface via Reaction-Induced Reconstruction for CO₂ Hydrogenation to C₂₊ Hydrocarbons

Area of Science:

• Catalysis
• Materials Science
• Chemical Engineering

Background:

• Interfacial catalysts offer potential for CO2 hydrogenation to multicarbon products via synergistic C=O bond activation and C-C coupling.
• Controllable construction of such interfaces under reaction conditions is a significant challenge.

Purpose of the Study:

• To engineer a Cu(0)-Co2C interfacial architecture using reaction-induced reconstruction for enhanced CO2 hydrogenation.
• To elucidate the carburization mechanism and interfacial synergy in Co-Cu catalysts for CO2 valorization.

Main Methods:

• Employing a reaction-induced reconstruction strategy to form Cu(0)-Co2C interfaces from Co-Cu oxides during CO2 hydrogenation.
• Investigating the outside-in carburization mechanism and its dependence on Co(0)-Cu(0) interactions.
• Characterizing catalytic performance, including C2+ hydrocarbon selectivity and yield.

Main Results:

• Achieved a significant increase in C2+ hydrocarbon selectivity from ~1% to ~60% with the optimized Cu(0)-Co2C catalyst.
• Demonstrated a record C2+ yield of 19.4 mmol g-1(Co2C) h-1 at 300 °C and 3 MPa, outperforming the K-Co2C reference.
• Identified that the Cu(0)-Co2C interface promotes CO*-mediated pathways and enhances CH2* coupling.

Conclusions:

• Established a rational methodology for designing in situ-evolved metal-carbide interfaces for CO2 valorization.
• Demonstrated the effectiveness of Cu(0)-Co2C interfacial catalysts in improving CO2 hydrogenation efficiency.
• Unraveled dynamic reconstruction mechanisms and interfacial synergy in Co-Cu catalytic systems.